AbstractAn intelligent process for developing electromagnetic interference (EMI) shielding composites is imperative to eliminate the escalating pollution of electromagnetic waves (EMWs). Meanwhile, integrating porous and/or layered structures with polymers is demonstrated as an effective approach. Herein, expert knowledge serves as the guidance of the Simulation‐First Strategy in designing shielding structures that incorporate MXene bubble wrap‐like aerogels (MBa‐bA), characterized by distinct bubble diameters a and densities b. The simulated EMI shielding efficiency (EMI SE) of corresponding MBa‐bA/polyethylene glycol (MBa‐bAP) composites is predicted through the finite element analysis (FEA) simulation. Subsequently, the MBa‐bAP composites are fabricated by template methods and exhibit an outstanding EMI SE of up to 83.1 dB and an ultrahigh SE of absorption (SEA) of 75.1 dB in X band at a = 10 µm and b = 0.50, perfectly aligning with the simulation outcomes. Combined with macro‐scale FEA simulation and experimental evidence, the pronounced EMWs attenuation effect, heat storage/release, and mechanical performances of MBa‐bAP composites are unequivocally substantiated. Based on these, this work proves the feasibility of the intelligent development strategy and provides a research basis for developing advanced EMI shielding materials directed by expert knowledge.
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